A nested sintering substrate and a sintering preparation process thereof

Abstract

This invention relates to the field of substrates, specifically to a nested sintered substrate and its sintering preparation process, which addresses the problems of high overall loss and poor overall mechanical properties of traditional nested sintered substrates. This nested sintered substrate utilizes a hollow cylindrical ceramic green body to provide a high dielectric constant and low dielectric loss, which is beneficial for device miniaturization and reduces signal energy loss, thereby maintaining signal integrity and making it suitable for high-speed data transmission, improving signal quality and bandwidth. A solid cylindrical ferrite green body provides specific saturation magnetization, achieving good magnetic shielding and reducing electromagnetic interference, thus reducing electromagnetic wave transmission loss in matched microstrip lines. The synergistic effect of these two factors significantly reduces the overall loss of the nested sintered substrate. Furthermore, a high-performance composite adhesive is used to bond the two components, significantly improving the interfacial bonding strength and thus enhancing the overall mechanical properties of the nested sintered substrate.

Description

Technical Field

[0001] This invention relates to the field of substrates, specifically to a nested sintered substrate and its sintering preparation process. Background Technology

[0002] With the development of modern electronic technology, the demand for high-performance and high-reliability electronic components is increasing. Traditional substrates, mostly made of a single material, are widely used, including ceramics and ferrites. Ceramic materials are favored for their excellent insulation and mechanical strength, while ferrite materials excel in high-frequency applications due to their high permeability and low loss characteristics. However, single-material substrates suffer from limited performance characteristics. Therefore, combining ceramics and ferrites to form nested structure substrates can effectively compensate for their respective shortcomings, fully leverage the advantages of both materials, and meet the more demanding application scenarios.

[0003] Currently, nested structure substrates mainly adopt co-firing technology, in which ferrite materials and dielectric ceramic materials are sintered in the same sintering process to achieve the combination of the two materials. However, the two materials have different sintering temperatures and coefficients of thermal expansion, which makes it impossible for them to be tightly connected after co-firing. The interface bonding strength between the two is low, resulting in poor overall performance of the nested sintered substrate.

[0004] Therefore, in order to improve the overall performance of nested sintered substrates, it is of great significance to develop a nested sintered substrate and its sintering preparation process. Summary of the Invention

[0005] In order to overcome the above-mentioned technical problems, the present invention aims to provide a nested sintered substrate and its sintering preparation process, which solves the problems of high overall loss and low overall mechanical properties of traditional nested sintered substrates, making it difficult to meet the ever-increasing performance requirements of modern electronic devices.

[0006] The objective of this invention can be achieved through the following technical solutions:

[0007] A nested sintered substrate is made by sintering a hollow cylindrical ceramic green body with a glue-coated solid cylindrical ferrite green body nested inside it.

[0008] Among them, the coated solid cylindrical ferrite preform is made by coating the outside of the solid cylindrical ferrite preform with high-performance composite adhesive;

[0009] The high-performance composite adhesive is prepared by the following steps:

[0010] Step s1: Weigh out 35-40 parts of organosilicon phenyl epoxy resin, 26-32 parts of inorganic filler adhesive, 18-22 parts of curing agent, 1.2-2.8 parts of reinforcing material and 17-21 parts of phenyl glycidyl ether according to the weight ratio, and set aside.

[0011] Step s2: Mix the organosilicon phenyl epoxy resin, inorganic filler adhesive, curing agent, reinforcing agent and phenyl glycidyl ether evenly to obtain a high-performance composite adhesive.

[0012] In a preferred embodiment of the present invention, the organosilicon phenyl epoxy resin in step s1 is prepared by the following steps:

[0013] Step a1: Add 4-vinylphenol, epichlorohydrin, and benzyltriethylammonium chloride to a three-necked flask equipped with a stirrer, thermometer, gas delivery tube, and constant pressure dropping funnel. Purge with nitrogen for protection and stir the reaction at 25-30℃ and 200-300 r / min for 5-10 min. Then raise the temperature to 105-115℃ and continue stirring for 2-3 h. Then lower the temperature to 80-85℃ and add sodium hydroxide solution dropwise while stirring, controlling the dropping rate to 1-2 drops / s. After the addition is complete, continue stirring for 4-5 h. After the reaction is complete, cool the reaction product to room temperature, then remove the solvent by rotary evaporation. Wash with distilled water 3-5 times, then place in a vacuum drying oven and dry at 70-80℃ for 3-4 h to obtain epoxy-alkenylbenzene.

[0014] Step a2: Add epoxy alkenylbenzene, tetramethyldisiloxane, Karstedt catalyst and toluene to a three-necked flask equipped with a stirrer and thermometer. Stir the reaction at 25-30℃ and 200-300 r / min for 30-40 min. Then raise the temperature to 100-110℃ and continue stirring for 10-15 h. After the reaction is completed, cool the reaction product to room temperature and then remove the solvent by rotary evaporation to obtain organosilicon phenyl epoxy resin.

[0015] In a preferred embodiment of the present invention, the ratio of 4-vinylphenol, epichlorohydrin, benzyltriethylammonium chloride and sodium hydroxide solution in step a1 is 5-6g: 18-20g: 0.15-0.25g: 13-15mL.

[0016] In a preferred embodiment of the present invention, the sodium hydroxide solution in step a1 has a mass fraction of 25-30%.

[0017] In a preferred embodiment of the present invention, the ratio of epoxy-alkenylbenzene, tetramethyldisiloxane, Karstedt catalyst and toluene in step a2 is 10 mmol: 20 mmol: 0.2-0.3 mL: 60-70 mL.

[0018] In a preferred embodiment of the present invention, the inorganic filler adhesive in step s1 is a mixture of alumina, boron carbide and aluminum powder in a mass ratio of 1:3-3.6:1.5-1.8.

[0019] In a preferred embodiment of the present invention, the curing agent in step s1 is polyamide curing agent 651.

[0020] In a preferred embodiment of the present invention, the reinforcing material in step s1 is a high-purity single-walled carbon nanotube of type XFS05.

[0021] As a preferred embodiment of the present invention, a sintering preparation process for a nested sintered substrate includes the following steps:

[0022] Step 1: Add high dielectric ceramic raw materials, zirconium dioxide grinding balls, and anhydrous ethanol to a ball mill at a material:ball:liquid mass ratio of 1:2:2. Ball mill for 6-8 hours at a ball milling rate of 200-300 r / min. Then place the mixture in a vacuum drying oven and dry it at a temperature of 70-80℃ for 2-3 hours. After that, place it in a muffle furnace and dry it at a temperature of 900-950℃ for 2-3 hours. After cooling, remove the mixture to obtain primary ceramic grinding powder.

[0023] Step 2: Add the primary ceramic grinding powder, zirconium dioxide grinding balls, and anhydrous ethanol to a ball mill at a material:ball:liquid mass ratio of 1:2:2. Ball mill for 10-12 hours at a grinding rate of 200-300 r / min. Then place the mixture in a vacuum drying oven and dry it at a temperature of 90-100℃ for 3-5 hours. Finally, grind the mixture through a 100-mesh sieve to obtain ceramic raw material powder.

[0024] Step 3: Add the high-dielectric ferrite raw material, zirconium dioxide grinding balls, and anhydrous ethanol into a ball mill at a material:ball:liquid mass ratio of 1:2:2. Ball mill for 6-8 hours at a ball milling rate of 200-300 r / min. Then place it in a vacuum drying oven and dry it at a temperature of 70-80℃ for 2-3 hours. After that, place it in a muffle furnace and dry it at a temperature of 825-855℃ for 2-3 hours. After cooling, remove it to obtain primary ferrite grinding powder.

[0025] Step 4: Add the ferrite grinding powder, zirconium dioxide grinding balls, and anhydrous ethanol to the ball mill at a mass ratio of 1:2:2 (material:ball:liquid). Ball mill for 10-12 hours at a grinding rate of 200-300 r / min. Then place the mixture in a vacuum drying oven and dry it at 90-100℃ for 3-5 hours. Finally, grind the mixture through a 100-mesh sieve to obtain the ferrite raw material powder.

[0026] Step 5: Mix the ceramic raw material powder and polyvinyl alcohol evenly, and then press them into hollow cylindrical ceramic green bodies under a pressure of 150-200 MPa. Mix the ferrite raw material powder and polyvinyl alcohol evenly, and then press them into solid cylindrical ferrite green bodies under a pressure of 150-200 MPa. Then, evenly coat the surface of the solid cylindrical ferrite green body with high-performance composite adhesive to obtain an adhesive-coated solid cylindrical ferrite green body. Then, nest the adhesive-coated solid cylindrical ferrite green body inside the hollow cylindrical ceramic green body, and then place it in a muffle furnace. Sinter at a temperature of 500-700℃ for 24-48 hours, and then raise the temperature to 1250-1300℃ at a rate of 3-5℃ / min for 6-12 hours. Then, cool it with the furnace to obtain the nested sintered substrate.

[0027] In a preferred embodiment of the present invention, the high dielectric ceramic raw material in step one is composed of calcium carbonate, copper oxide, titanium dioxide, magnesium oxide, zinc oxide and tungsten trioxide mixed in a molar ratio of 1-1.2:3-3.3:4-4.5:7-8:2.5-2.7:0.5-0.6.

[0028] In a preferred embodiment of the present invention, the high-dielectric ferrite raw material in step three is a mixture of bismuth trioxide, yttrium trioxide, calcium carbonate, tin oxide, manganese carbonate and ferric oxide in a molar ratio of 6-7:3-3.6:12-15:0.1-0.12:0.09-0.11:21-25.

[0029] In a preferred embodiment of the present invention, the mass ratio of ceramic raw material powder to polyvinyl alcohol in step five is 95:5-6.

[0030] In a preferred embodiment of the present invention, the mass ratio of ferrite raw material powder to polyvinyl alcohol in step five is 90:10-12.

[0031] In a preferred embodiment of the present invention, the polyvinyl alcohol in step five is PVA 17-88.

[0032] Compared with the prior art, the beneficial effects of the present invention are:

[0033] This nested sintered substrate utilizes a hollow cylindrical ceramic green body to provide high dielectric constant and low dielectric loss, which is beneficial for device miniaturization and reduces signal energy loss, thereby maintaining signal integrity and making it suitable for high-speed data transmission, improving signal quality and bandwidth. A solid cylindrical ferrite green body provides specific saturation magnetization, achieving good magnetic shielding and reducing electromagnetic interference. This further reduces electromagnetic wave transmission loss in the matched microstrip line. The synergistic effect of these two factors significantly reduces the overall loss of the nested sintered substrate. Furthermore, a high-performance composite adhesive is used to bond the two components, significantly improving the interfacial bonding strength and thus enhancing the overall mechanical properties of the nested sintered substrate. It can withstand certain external impacts and vibrations, improving the reliability and service life of the nested sintered substrate. Moreover, the sintering process is simple, easy to industrialize, and reduces production costs.

[0034] In the process of preparing the nested sintered substrate, a high-performance composite adhesive was first prepared. This involved reacting 4-vinylphenol with epichlorohydrin, where the hydroxyl groups on 4-vinylphenol underwent a ring-opening-ring-closing reaction with epichlorohydrin, introducing epoxy groups to obtain epoxy-alkenylbenzene. Subsequently, the epoxy-alkenylbenzene reacted with tetramethyldisiloxane, where the alkenyl groups on the epoxy-alkenylbenzene and the Si-H groups on the tetramethyldisiloxane underwent a hydrosilylation reaction to obtain organosilicon phenyl epoxy resin. Then, using the organosilicon phenyl epoxy resin as an organic adhesive, a compound of alumina, boron carbide, and aluminum powder as an inorganic filler adhesive, and high-purity single-walled carbon nanotubes as a reinforcing material, along with a curing agent and phenyl glycidyl ether, a high-performance composite adhesive was obtained. Silicon-phenyl epoxy resin utilizes phenyl groups and Si-O bonds to impart excellent high-temperature resistance, thus facilitating better synergistic effects with inorganic filler adhesives. Boron carbide and aluminum powder in the inorganic filler adhesive react and melt upon high-temperature heating, effectively filling defects and pores caused by the decomposition of organic adhesives. Alumina further enhances high-temperature stability and skeletal support, while reinforcing materials improve the overall mechanical strength of the adhesive. Therefore, the synergistic effect of organic adhesives, inorganic filler adhesives, and reinforcing materials endows the high-performance composite adhesive with excellent mechanical properties, enabling tight bonding of hollow cylindrical ceramic green bodies and solid cylindrical ferrite green bodies, thereby improving the overall mechanical properties of nested sintered substrates. Attached Figure Description

[0035] To facilitate understanding by those skilled in the art, the present invention will be further described below with reference to the accompanying drawings.

[0036] Figure 1 This is a schematic flowchart of the sintering preparation process of a nested sintered substrate according to the present invention. Detailed Implementation

[0037] To enable those skilled in the art to better understand the present invention, the technical solutions of the present invention will be clearly and completely described below with reference to the accompanying drawings of the embodiments of the present invention. Obviously, the described embodiments are only some embodiments of the present invention, and not all embodiments. Based on the embodiments of the present invention, all other embodiments obtained by those skilled in the art without creative effort are within the scope of protection of the present invention.

[0038] Example 1:

[0039] Please see Figure 1 As shown, this embodiment illustrates a sintering fabrication process for nested sintered substrates, comprising the following steps:

[0040] Step 1: High-dielectric ceramic raw material, zirconium dioxide grinding balls, and anhydrous ethanol are added to a ball mill at a material:ball:liquid mass ratio of 1:2:2. The mixture is ball-milled for 6 hours at a milling rate of 200 r / min. After milling, it is placed in a vacuum drying oven and dried at 70°C for 2 hours. Then, it is placed in a muffle furnace and dried at 900°C for 2 hours. After cooling, the powder is removed to obtain primary ceramic grinding powder. The high-dielectric ceramic raw material is composed of calcium carbonate, copper oxide, titanium dioxide, magnesium oxide, zinc oxide, and tungsten trioxide mixed in a molar ratio of 1:3:4:7:2.5:0.5.

[0041] Step 2: Add the primary ceramic grinding powder, zirconium dioxide grinding balls, and anhydrous ethanol to the ball mill at a mass ratio of 1:2:2 (material:ball:liquid). Grind the mixture for 10 hours at a ball milling rate of 200 r / min. Then, place it in a vacuum drying oven and dry it at 90℃ for 3 hours. Finally, grind the mixture through a 100-mesh sieve to obtain the ceramic raw material powder.

[0042] Step 3: Add high-dielectric ferrite raw material, zirconium dioxide grinding balls, and anhydrous ethanol to a ball mill at a material:ball:liquid mass ratio of 1:2:2. Ball mill for 6 hours at a milling rate of 200 r / min. Then place in a vacuum drying oven and dry at 70°C for 2 hours. After that, place in a muffle furnace and dry at 825°C for 2 hours. After cooling, remove the powder to obtain primary ferrite grinding powder. The high-dielectric ferrite raw material is composed of bismuth trioxide, yttrium trioxide, calcium carbonate, tin oxide, manganese carbonate, and ferric oxide in a molar ratio of 6:3:12:0.1:0.09:21.

[0043] Step 4: Add the ferrite grinding powder, zirconium dioxide grinding balls, and anhydrous ethanol into the ball mill at a material:ball:liquid mass ratio of 1:2:2. Ball mill for 10 hours at a ball milling rate of 200 r / min. Then place it in a vacuum drying oven and dry it at a temperature of 90℃ for 3 hours. Finally, grind it through a 100-mesh sieve to obtain ferrite raw material powder.

[0044] Step 5: Mix the ceramic raw material powder and PVA 17-88 polyvinyl alcohol at a mass ratio of 95:5 until homogeneous. Then, press the mixture under a pressure of 150MPa to form a hollow cylindrical ceramic green body with an inner diameter of 5.03mm, an outer diameter of 10mm, and a height of 5mm. (The text then repeats the steps for the next step, which is unclear without further context.) Polyvinyl alcohol 17-88 was mixed uniformly at a mass ratio of 90:10, and then pressed into a solid cylindrical ferrite green body with a diameter of 5 mm and a height of 5 mm under a pressure of 150 MPa. Then, a high-performance composite adhesive with a thickness of 0.1 mm was uniformly coated on the surface of the solid cylindrical ferrite green body to obtain an adhesive-coated solid cylindrical ferrite green body. The adhesive-coated solid cylindrical ferrite green body was then nested and assembled inside a hollow cylindrical ceramic green body. It was then placed in a muffle furnace and sintered at a temperature of 500℃ for 24 h. After that, the temperature was increased to 1250℃ at a rate of 3℃ / min and sintered for 6 h. After that, it was cooled with the furnace to obtain a nested sintered substrate.

[0045] The high-performance composite adhesive is prepared by the following steps:

[0046] Step s11: Add 5g of 4-vinylphenol, 18g of epichlorohydrin and 0.15g of benzyltriethylammonium chloride to a three-necked flask equipped with a stirrer, thermometer, gas delivery tube and constant pressure dropping funnel. Purge with nitrogen and stir at 25℃ and 200r / min for 5min. Then raise the temperature to 105℃ and continue stirring for 2h. Then lower the temperature to 80℃ and add 13mL of 25% sodium hydroxide solution dropwise while stirring, controlling the dropping rate to 1 drop / s. After the addition is complete, continue stirring for 4h. After the reaction is complete, cool the reaction product to room temperature, then remove the solvent by rotary evaporation, wash three times with distilled water, and then place it in a vacuum drying oven and dry at 70℃ for 3h to obtain epoxy-alkenylbenzene.

[0047] Step s12: 10 mmol of epoxy alkenylbenzene, 20 mmol of tetramethyldisiloxane, 0.2 mL of Karstedt catalyst and 60 mL of toluene were added to a three-necked flask equipped with a stirrer and a thermometer. The mixture was stirred at 25 °C and 200 r / min for 30 min. Then the temperature was raised to 100 °C and the mixture was stirred for 10 h. After the reaction was completed, the reaction product was cooled to room temperature and the solvent was removed by rotary evaporation to obtain organosilicon phenyl epoxy resin.

[0048] Step s13: Weigh out 35 parts by weight of organosilicon phenyl epoxy resin, 26 parts by weight of inorganic filler binder, 18 parts by weight of curing agent, 1.2 parts by weight of reinforcing material, and 17 parts by weight of phenyl glycidyl ether, and set aside; wherein, the inorganic filler binder is a mixture of alumina, boron carbide, and aluminum powder in a mass ratio of 1:3:1.5; wherein, the curing agent is polyamide curing agent 651; wherein, the reinforcing material is high-purity single-walled carbon nanotubes of model XFS05;

[0049] Step s14: Mix the organosilicon phenyl epoxy resin, inorganic filler adhesive, curing agent, reinforcing agent and phenyl glycidyl ether evenly to obtain a high-performance composite adhesive.

[0050] Example 2:

[0051] Please see Figure 1 As shown, this embodiment illustrates a sintering fabrication process for nested sintered substrates, comprising the following steps:

[0052] Step 1: High-dielectric ceramic raw material, zirconium dioxide grinding balls, and anhydrous ethanol are added to a ball mill at a material:ball:liquid mass ratio of 1:2:2. The mixture is ball-milled for 7 hours at a milling rate of 250 r / min. Afterward, it is placed in a vacuum drying oven and dried at 75°C for 2.5 hours. Then, it is placed in a muffle furnace and dried at 925°C for 2.5 hours. Finally, it is cooled and removed to obtain primary ceramic grinding powder. The high-dielectric ceramic raw material is composed of calcium carbonate, copper oxide, titanium dioxide, magnesium oxide, zinc oxide, and tungsten trioxide mixed in a molar ratio of 1.1:3.1:4.3:7.5:2.6:0.55.

[0053] Step 2: Add the primary ceramic grinding powder, zirconium dioxide grinding balls, and anhydrous ethanol to the ball mill at a mass ratio of 1:2:2 (material:ball:liquid). Grind the mixture for 11 hours at a ball milling rate of 250 r / min. Then, place it in a vacuum drying oven and dry it at 95℃ for 4 hours. Finally, grind the mixture through a 100-mesh sieve to obtain the ceramic raw material powder.

[0054] Step 3: Add high-dielectric ferrite raw material, zirconium dioxide grinding balls, and anhydrous ethanol to a ball mill at a material:ball:liquid mass ratio of 1:2:2. Ball mill for 7 hours at a milling rate of 250 r / min. Then place in a vacuum drying oven and dry at 75°C for 2.5 hours. After that, place in a muffle furnace and dry at 840°C for 2.5 hours. After cooling, remove the powder to obtain primary ferrite grinding powder. The high-dielectric ferrite raw material is composed of bismuth trioxide, yttrium trioxide, calcium carbonate, tin oxide, manganese carbonate, and ferric oxide in a molar ratio of 6.5:3.3:13.5:0.11:0.1:23.

[0055] Step 4: Add the ferrite grinding powder, zirconium dioxide grinding balls, and anhydrous ethanol into the ball mill at a mass ratio of 1:2:2 (material:ball:liquid). Ball mill for 11 hours at a grinding rate of 250 r / min. Then place the mixture in a vacuum drying oven and dry it at 95℃ for 4 hours. Finally, grind the mixture through a 100-mesh sieve to obtain the ferrite raw material powder.

[0056] Step 5: Mix the ceramic raw material powder and PVA 17-88 polyvinyl alcohol at a mass ratio of 95:5.5 until homogeneous. Then, press the mixture under a pressure of 175 MPa to form a hollow cylindrical ceramic green body with an inner diameter of 5.03 mm, an outer diameter of 10 mm, and a height of 5 mm. (The text then repeats the steps for the next step, which is unclear without further context.) Polyvinyl alcohol 17-88 was mixed uniformly at a mass ratio of 90:11, and then pressed into a solid cylindrical ferrite green body with a diameter of 5 mm and a height of 5 mm under a pressure of 175 MPa. Then, a high-performance composite adhesive with a thickness of 0.15 mm was uniformly coated on the surface of the solid cylindrical ferrite green body to obtain an adhesive-coated solid cylindrical ferrite green body. The adhesive-coated solid cylindrical ferrite green body was then nested and assembled inside a hollow cylindrical ceramic green body. It was then placed in a muffle furnace and sintered at a temperature of 600℃ for 36 h. After that, the temperature was increased to 1275℃ at a rate of 4℃ / min and sintered for 9 h. After that, it was cooled with the furnace to obtain a nested sintered substrate.

[0057] The high-performance composite adhesive is prepared by the following steps:

[0058] Step s11: Add 5.5g of 4-vinylphenol, 19g of epichlorohydrin, and 0.20g of benzyltriethylammonium chloride to a three-necked flask equipped with a stirrer, thermometer, gas delivery tube, and constant pressure dropping funnel. Purge with nitrogen for protection and stir at 28℃ and 250r / min for 7min. Then raise the temperature to 110℃ and continue stirring for 2.5h. After cooling to 82℃, add 14mL of 28% sodium hydroxide solution dropwise while stirring, controlling the dropping rate to 1 drop / s. After the addition is complete, continue stirring for 4.5h. After the reaction is complete, cool the reaction product to room temperature, then remove the solvent by rotary evaporation. Wash with distilled water 4 times, then place in a vacuum drying oven and dry at 75℃ for 3.5h to obtain epoxy-alkenylbenzene.

[0059] Step s12: 10 mmol of epoxy alkenylbenzene, 20 mmol of tetramethyldisiloxane, 0.25 mL of Karstedt catalyst and 65 mL of toluene were added to a three-necked flask equipped with a stirrer and a thermometer. The mixture was stirred at 28 °C and 250 r / min for 35 min. Then the temperature was raised to 105 °C and the mixture was stirred for 12 h. After the reaction was completed, the reaction product was cooled to room temperature and the solvent was removed by rotary evaporation to obtain organosilicon phenyl epoxy resin.

[0060] Step s13: Weigh out 38 parts by weight of organosilicon phenyl epoxy resin, 29 parts by weight of inorganic filler binder, 20 parts by weight of curing agent, 2 parts by weight of reinforcing material, and 19 parts by weight of phenyl glycidyl ether, and set aside; wherein, the inorganic filler binder is a mixture of alumina, boron carbide, and aluminum powder in a mass ratio of 1:3.3:1.7; wherein, the curing agent is polyamide curing agent 651; wherein, the reinforcing material is high-purity single-walled carbon nanotubes of model XFS05;

[0061] Step s14: Mix the organosilicon phenyl epoxy resin, inorganic filler adhesive, curing agent, reinforcing agent and phenyl glycidyl ether evenly to obtain a high-performance composite adhesive.

[0062] Example 3:

[0063] Please see Figure 1 As shown, this embodiment illustrates a sintering fabrication process for nested sintered substrates, comprising the following steps:

[0064] Step 1: High-dielectric ceramic raw material, zirconium dioxide grinding balls, and anhydrous ethanol are added to a ball mill at a material:ball:liquid mass ratio of 1:2:2. The mixture is ball-milled for 8 hours at a milling rate of 300 r / min. After milling, it is placed in a vacuum drying oven and dried at 80°C for 3 hours. Then, it is placed in a muffle furnace and dried at 950°C for 3 hours. After cooling, the powder is removed to obtain primary ceramic grinding powder. The high-dielectric ceramic raw material is composed of calcium carbonate, copper oxide, titanium dioxide, magnesium oxide, zinc oxide, and tungsten trioxide mixed in a molar ratio of 1.2:3.3:4.5:8:2.7:0.6.

[0065] Step 2: Add the primary ceramic grinding powder, zirconium dioxide grinding balls, and anhydrous ethanol to a ball mill at a material:ball:liquid mass ratio of 1:2:2. Ball mill for 12 hours at a grinding rate of 300 r / min. Then place the mixture in a vacuum drying oven and dry it at 100℃ for 5 hours. Finally, grind the mixture through a 100-mesh sieve to obtain ceramic raw material powder.

[0066] Step 3: Add high-dielectric ferrite raw material, zirconium dioxide grinding balls, and anhydrous ethanol to a ball mill at a material:ball:liquid mass ratio of 1:2:2. Ball mill for 8 hours at a milling rate of 300 r / min. Then place in a vacuum drying oven and dry at 80°C for 3 hours. After that, place in a muffle furnace and dry at 855°C for 3 hours. After cooling, remove the powder to obtain primary ferrite grinding powder. The high-dielectric ferrite raw material is composed of bismuth trioxide, yttrium trioxide, calcium carbonate, tin oxide, manganese carbonate, and ferric oxide in a molar ratio of 7:3.6:15:0.12:0.11:25.

[0067] Step 4: Add the ferrite grinding powder, zirconium dioxide grinding balls, and anhydrous ethanol to the ball mill at a mass ratio of 1:2:2 (material:ball:liquid). Ball mill for 12 hours at a grinding rate of 300 r / min. Then place the mixture in a vacuum drying oven and dry it at 100℃ for 5 hours. Finally, grind the mixture through a 100-mesh sieve to obtain the ferrite raw material powder.

[0068] Step 5: Mix the ceramic raw material powder and PVA 17-88 polyvinyl alcohol at a mass ratio of 95:6 until homogeneous. Then, press the mixture under a pressure of 200MPa to form a hollow cylindrical ceramic green body with an inner diameter of 5.03mm, an outer diameter of 10mm, and a height of 5mm. (The text then repeats the steps for the next step, which is unclear without further context.) Polyvinyl alcohol 17-88 was mixed uniformly at a mass ratio of 90:12, and then pressed into a solid cylindrical ferrite green body with a diameter of 5 mm and a height of 5 mm under a pressure of 200 MPa. Then, a high-performance composite adhesive with a thickness of 0.2 mm was uniformly coated on the surface of the solid cylindrical ferrite green body to obtain an adhesive-coated solid cylindrical ferrite green body. The adhesive-coated solid cylindrical ferrite green body was then nested and assembled inside a hollow cylindrical ceramic green body. It was then placed in a muffle furnace and sintered at a temperature of 700℃ for 48 h. After that, the temperature was increased to 1300℃ at a rate of 5℃ / min and sintered for 12 h. After that, it was cooled with the furnace to obtain a nested sintered substrate.

[0069] The high-performance composite adhesive is prepared by the following steps:

[0070] Step s11: Add 6g of 4-vinylphenol, 20g of epichlorohydrin and 0.25g of benzyltriethylammonium chloride to a three-necked flask equipped with a stirrer, thermometer, gas delivery tube and constant pressure dropping funnel. Purge with nitrogen and stir for 10 min at 30℃ and 300 r / min. Then raise the temperature to 115℃ and continue stirring for 3 h. Then lower the temperature to 85℃ and add 15 mL of 30% sodium hydroxide solution dropwise while stirring, controlling the dropping rate to 2 drops / s. After the addition is complete, continue stirring for 5 h. After the reaction is complete, cool the reaction product to room temperature, then remove the solvent by rotary evaporation, wash 5 times with distilled water, and then place it in a vacuum drying oven and dry at 80℃ for 4 h to obtain epoxy-alkenylbenzene.

[0071] Step s12: 10 mmol of epoxy alkenylbenzene, 20 mmol of tetramethyldisiloxane, 0.3 mL of Karstedt catalyst and 70 mL of toluene were added to a three-necked flask equipped with a stirrer and a thermometer. The mixture was stirred at 30 °C and 300 r / min for 40 min. Then the temperature was raised to 110 °C and the mixture was stirred for 15 h. After the reaction was completed, the reaction product was cooled to room temperature and the solvent was removed by rotary evaporation to obtain organosilicon phenyl epoxy resin.

[0072] Step s13: Weigh out 40 parts by weight of organosilicon phenyl epoxy resin, 32 parts by weight of inorganic filler binder, 22 parts by weight of curing agent, 2.8 parts by weight of reinforcing material, and 21 parts by weight of phenyl glycidyl ether, and set aside; wherein, the inorganic filler binder is a mixture of alumina, boron carbide, and aluminum powder in a mass ratio of 1:3.6:1.8; wherein, the curing agent is polyamide curing agent 651; wherein, the reinforcing material is high-purity single-walled carbon nanotubes of model XFS05;

[0073] Step s14: Mix the organosilicon phenyl epoxy resin, inorganic filler adhesive, curing agent, reinforcing agent and phenyl glycidyl ether evenly to obtain a high-performance composite adhesive.

[0074] Comparative Example 1:

[0075] The difference between this comparative example and Example 3 is that the high-performance composite adhesive is prepared by the following steps:

[0076] Step s11: Weigh out 40 parts of E-44 epoxy resin, 22 parts of curing agent, and 21 parts of phenyl glycidyl ether according to the weight ratio, and set aside; wherein, the curing agent is polyamide curing agent 651;

[0077] Step s14: Mix E-44 epoxy resin, curing agent and phenyl glycidyl ether evenly to obtain high-performance composite adhesive.

[0078] Comparative Example 2:

[0079] The difference between this comparative example and Example 3 is that the high-performance composite adhesive is prepared by the following steps:

[0080] Step s11: Weigh out 40 parts of E-44 epoxy resin, 22 parts of curing agent, 2.8 parts of reinforcing material and 21 parts of phenyl glycidyl ether according to the weight ratio, and set aside; wherein, the curing agent is polyamide curing agent 651; wherein, the reinforcing material is high-purity single-walled carbon nanotubes of model XFS05;

[0081] Step s12: Mix E-44 epoxy resin, curing agent, reinforcing agent and phenyl glycidyl ether evenly to obtain high-performance composite adhesive.

[0082] Comparative Example 3:

[0083] The difference between this comparative example and Example 3 is that the high-performance composite adhesive is prepared by the following steps:

[0084] Step s11: Weigh out 40 parts by weight of E-44 epoxy resin, 32 parts by weight of inorganic filler adhesive, 22 parts by weight of curing agent, and 21 parts by weight of phenyl glycidyl ether, and set aside; wherein, the inorganic filler adhesive is a mixture of alumina, boron carbide, and aluminum powder in a mass ratio of 1:3.6:1.8; wherein, the curing agent is polyamide curing agent 651;

[0085] Step s12: Mix E-44 epoxy resin, inorganic filler adhesive, curing agent and phenyl glycidyl ether evenly to obtain high-performance composite adhesive.

[0086] Comparative Example 4:

[0087] The difference between this comparative example and Example 3 is that the high-performance composite adhesive is prepared by the following steps:

[0088] Step s11: Weigh out 40 parts by weight of E-44 epoxy resin, 32 parts by weight of inorganic filler adhesive, 22 parts by weight of curing agent, 2.8 parts by weight of reinforcing material, and 21 parts by weight of phenyl glycidyl ether, and set aside; wherein, the inorganic filler adhesive is a mixture of alumina, boron carbide, and aluminum powder in a mass ratio of 1:3.6:1.8; wherein, the curing agent is polyamide curing agent 651; wherein, the reinforcing material is high-purity single-walled carbon nanotubes of model XFS05;

[0089] Step s12: Mix E-44 epoxy resin, inorganic filler adhesive, curing agent, reinforcing agent and phenyl glycidyl ether evenly to obtain high-performance composite adhesive.

[0090] Comparative Example 5:

[0091] The difference between this comparative example and Example 3 is that the high-performance composite adhesive is prepared by the following steps:

[0092] Step s11: Add 6g of 4-vinylphenol, 20g of epichlorohydrin and 0.25g of benzyltriethylammonium chloride to a three-necked flask equipped with a stirrer, thermometer, gas delivery tube and constant pressure dropping funnel. Purge with nitrogen and stir for 10 min at 30℃ and 300 r / min. Then raise the temperature to 115℃ and continue stirring for 3 h. Then lower the temperature to 85℃ and add 15 mL of 30% sodium hydroxide solution dropwise while stirring, controlling the dropping rate to 2 drops / s. After the addition is complete, continue stirring for 5 h. After the reaction is complete, cool the reaction product to room temperature, then remove the solvent by rotary evaporation, wash 5 times with distilled water, and then place it in a vacuum drying oven and dry at 80℃ for 4 h to obtain epoxy-alkenylbenzene.

[0093] Step s12: 10 mmol of epoxy alkenylbenzene, 20 mmol of tetramethyldisiloxane, 0.3 mL of Karstedt catalyst and 70 mL of toluene were added to a three-necked flask equipped with a stirrer and a thermometer. The mixture was stirred at 30 °C and 300 r / min for 40 min. Then the temperature was raised to 110 °C and the mixture was stirred for 15 h. After the reaction was completed, the reaction product was cooled to room temperature and the solvent was removed by rotary evaporation to obtain organosilicon phenyl epoxy resin.

[0094] Step s13: Weigh out 40 parts by weight of organosilicon phenyl epoxy resin, 22 parts by weight of curing agent and 21 parts by weight of phenyl glycidyl ether, and set aside; wherein, the curing agent is polyamide curing agent 651;

[0095] Step s14: Mix the organosilicon phenyl epoxy resin, curing agent and phenyl glycidyl ether evenly to obtain a high-performance composite adhesive.

[0096] The performance of the nested sintered substrates of Examples 1-3 and Comparative Examples 1-5 was tested. The dielectric constant and dielectric loss at the resonant frequency of 9 GHz were tested, and the specific saturation magnetization was tested. The interfacial bonding strength between the solid cylindrical ferrite green body and the hollow cylindrical ceramic green body was evaluated by shear strength testing.

[0097] The test results are shown in the table below:

[0098]

[0099] Referring to the data in the table above, and based on the comparison between Examples 1-3 and Comparative Examples 1-5, the dielectric properties, magnetic properties, and mechanical properties of the nested sintered substrate of this application can be determined.

[0100] In the description of this specification, references to terms such as "an embodiment," "example," "specific example," etc., indicate that a specific feature, structure, material, or characteristic described in connection with that embodiment or example is included in at least one embodiment or example of the invention. In this specification, illustrative expressions of the above terms do not necessarily refer to the same embodiment or example. Furthermore, the specific features, structures, materials, or characteristics described may be combined in any suitable manner in one or more embodiments or examples.

[0101] The above description is merely an example and illustration of the present invention. Those skilled in the art can make various modifications or additions to the specific embodiments described or use similar methods to replace them, as long as they do not deviate from the invention or exceed the scope defined in this application, they should all fall within the protection scope of the present invention.

Claims

1. A nested sintered substrate, characterized by, It is made by sintering a hollow cylindrical ceramic green body with a solid cylindrical ferrite green body coated with adhesive inside. Among them, the coated solid cylindrical ferrite preform is made by coating the outside of the solid cylindrical ferrite preform with high-performance composite adhesive; The high-performance composite adhesive is prepared by the following steps: Step s1: Weigh out 35-40 parts of organosilicon phenyl epoxy resin, 26-32 parts of inorganic filler adhesive, 18-22 parts of curing agent, 1.2-2.8 parts of reinforcing material and 17-21 parts of phenyl glycidyl ether according to the weight ratio, and set aside. Step s2: Mix the organosilicon phenyl epoxy resin, inorganic filler adhesive, curing agent, reinforcing agent and phenyl glycidyl ether evenly to obtain a high-performance composite adhesive; The organosilicon phenyl epoxy resin in step s1 is prepared by the following steps: Step a1: 4-vinylphenol, epichlorohydrin and benzyltriethylammonium chloride were stirred and reacted. Then, sodium hydroxide solution was added dropwise while stirring. After the addition was completed, the reaction was continued to be stirred. After the reaction was completed, the reaction product was cooled, then evaporated by rotary evaporation, and then washed and dried to obtain epoxy-alkenylbenzene. Step a2: The epoxy alkenylbenzene, tetramethyldisiloxane, Karstedt catalyst and toluene are stirred and reacted. After the reaction is completed, the reaction product is cooled and then rotary evaporated to obtain organosilicon phenyl epoxy resin.

2. The nested sintered substrate of claim 1, wherein, In step a1, the ratio of 4-vinylphenol, epichlorohydrin, benzyltriethylammonium chloride, and sodium hydroxide solution is 5-6 g: 18-20 g: 0.15-0.25 g: 13-15 mL; the mass fraction of the sodium hydroxide solution is 25-30%; in step a2, the ratio of epoxyalkenylbenzene, tetramethyldisiloxane, Karstedt catalyst, and toluene is 10 mmol: 20 mmol: 0.2-0.3 mL: 60-70 mL.

3. The nested sintered substrate of claim 1, wherein, The inorganic filler adhesive in step s1 is a mixture of alumina, boron carbide, and aluminum powder in a mass ratio of 1:3-3.6:1.5-1.

8.

4. The nested sintered substrate of claim 1, wherein, The curing agent in step s1 is polyamide curing agent 651.

5. The nested sintered substrate of claim 1, wherein, The reinforcing material in step s1 is a high-purity single-walled carbon nanotube of model XFS05.

6. A sintering process for the production of nested sintered substrates as claimed in any one of claims 1 to 5, characterized in that, Includes the following steps: Step 1: Add high dielectric ceramic raw materials, zirconium dioxide grinding balls, and anhydrous ethanol to a ball mill at a material:ball:liquid mass ratio of 1:2:

2. Ball mill for 6-8 hours at a ball milling rate of 200-300 r / min. Then place the mixture in a vacuum drying oven and dry it at 70-80℃ for 2-3 hours. After that, place it in a muffle furnace and sinter it at 900-950℃ for 2-3 hours. After cooling, remove the mixture to obtain primary ceramic grinding powder. Step 2: Add the primary ceramic grinding powder, zirconium dioxide grinding balls, and anhydrous ethanol to a ball mill at a material:ball:liquid mass ratio of 1:2:

2. Ball mill for 10-12 hours at a grinding rate of 200-300 r / min. Then place the mixture in a vacuum drying oven and dry it at a temperature of 90-100℃ for 3-5 hours. Finally, grind the mixture through a 100-mesh sieve to obtain ceramic raw material powder. Step 3: Add the high-dielectric ferrite raw material, zirconium dioxide grinding balls, and anhydrous ethanol into a ball mill at a material:ball:liquid mass ratio of 1:2:

2. Ball mill for 6-8 hours at a ball milling rate of 200-300 r / min. Then place it in a vacuum drying oven and dry it at a temperature of 70-80℃ for 2-3 hours. After that, place it in a muffle furnace and sinter it at a temperature of 825-855℃ for 2-3 hours. After cooling, remove it to obtain primary ferrite grinding powder. Step 4: Add the ferrite grinding powder, zirconium dioxide grinding balls, and anhydrous ethanol to the ball mill at a mass ratio of 1:2:2 (material:ball:liquid). Ball mill for 10-12 hours at a grinding rate of 200-300 r / min. Then place the mixture in a vacuum drying oven and dry it at 90-100℃ for 3-5 hours. Finally, grind the mixture through a 100-mesh sieve to obtain the ferrite raw material powder. Step 5: Mix the ceramic raw material powder and polyvinyl alcohol evenly, and then press them into hollow cylindrical ceramic green bodies under a pressure of 150-200 MPa. Mix the ferrite raw material powder and polyvinyl alcohol evenly, and then press them into solid cylindrical ferrite green bodies under a pressure of 150-200 MPa. Then, evenly coat the surface of the solid cylindrical ferrite green body with high-performance composite adhesive to obtain an adhesive-coated solid cylindrical ferrite green body. Then, nest the adhesive-coated solid cylindrical ferrite green body inside the hollow cylindrical ceramic green body, and then place it in a muffle furnace. Sinter at a temperature of 500-700℃ for 24-48 hours, and then raise the temperature to 1250-1300℃ at a rate of 3-5℃ / min for 6-12 hours. Then, cool it with the furnace to obtain the nested sintered substrate.

7. The sintering process for nesting sintered substrates of claim 6, wherein, The high dielectric ceramic raw material mentioned in step one is composed of calcium carbonate, copper oxide, titanium dioxide, magnesium oxide, zinc oxide and tungsten trioxide mixed in a molar ratio of 1-1.2:3-3.3:4-4.5:7-8:2.5-2.7:0.5-0.

6.

8. The sintering process for nesting sintered substrates of claim 6, wherein, The high-dielectric ferrite raw material in step three is a mixture of bismuth trioxide, yttrium trioxide, calcium carbonate, tin oxide, manganese carbonate and ferric oxide in a molar ratio of 6-7:3-3.6:12-15:0.1-0.12:0.09-0.11:21-25.

9. The sintering process for nesting sintered substrates of claim 6, wherein, In step five, the mass ratio of ceramic raw material powder to polyvinyl alcohol is 95:5-6; the mass ratio of ferrite raw material powder to polyvinyl alcohol is 90:10-12; and the polyvinyl alcohol is PVA 17-88.

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